Saved in:
| Main Authors: | , , |
|---|---|
| Format: | Preprint |
| Published: |
2024
|
| Subjects: | |
| Online Access: | https://arxiv.org/abs/2408.13365 |
| Tags: |
Add Tag
No Tags, Be the first to tag this record!
|
| _version_ | 1866913478719045632 |
|---|---|
| author | Neville, Simon P. Jouybari, Martha Yaghoubi Schuurman, Michael S. |
| author_facet | Neville, Simon P. Jouybari, Martha Yaghoubi Schuurman, Michael S. |
| contents | Charge transfer is a fundamental phenomenon in biology and chemistry, and involves the movement of charge through a system driven by nuclear dynamics. Because of the involvement of nuclear motion, it is generally assumed that charge transfer will occur on a time-scale of some few tens-to-hundreds of femtoseconds. Using the example of ethylene excited to its $1sπ^{*}$ manifold, we demonstrate that ultrafast, few-femtosecond core-level charge transfer may occur following core-excitation, driven by the formation of electronic coherences by non-adiabatic dynamics. Here, transfer of core-electron density from one side of the molecule to the other is driven by a breakdown of the Born-Oppenheimer approximation, and results in core-hole localisation occuring within 5 fs, followed by core-hole delocalisation, all within the Auger decay window. These results serve to demonstrate that ultra-fast core-level charge transfer driven by nuclear dynamics may occur on the same timescale as purely electronic, i.e., charge migration, dynamics following core-excitation. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2408_13365 |
| institution | arXiv |
| publishDate | 2024 |
| record_format | arxiv |
| spellingShingle | Femtosecond Core-Level Charge Transfer Neville, Simon P. Jouybari, Martha Yaghoubi Schuurman, Michael S. Chemical Physics Charge transfer is a fundamental phenomenon in biology and chemistry, and involves the movement of charge through a system driven by nuclear dynamics. Because of the involvement of nuclear motion, it is generally assumed that charge transfer will occur on a time-scale of some few tens-to-hundreds of femtoseconds. Using the example of ethylene excited to its $1sπ^{*}$ manifold, we demonstrate that ultrafast, few-femtosecond core-level charge transfer may occur following core-excitation, driven by the formation of electronic coherences by non-adiabatic dynamics. Here, transfer of core-electron density from one side of the molecule to the other is driven by a breakdown of the Born-Oppenheimer approximation, and results in core-hole localisation occuring within 5 fs, followed by core-hole delocalisation, all within the Auger decay window. These results serve to demonstrate that ultra-fast core-level charge transfer driven by nuclear dynamics may occur on the same timescale as purely electronic, i.e., charge migration, dynamics following core-excitation. |
| title | Femtosecond Core-Level Charge Transfer |
| topic | Chemical Physics |
| url | https://arxiv.org/abs/2408.13365 |